The seismic performance of a self-centering precast reinforced concrete (RC) frame with shear walls was investigated in this paper. The lateral force resistance was provided by self-centering precast RC shear walls (SPCW), which utilize a combination of unbonded prestressed post-tensioned (PT) tendons and mild steel reinforcing bars for flexural resistance across base joints. The structures concentrated deformations at the bottom joints and the unbonded PT tendons provided the self-centering restoring force. A 1/3-scale model of a five-story self-centering RC frame with shear walls was designed and tested on a shake-table under a series of bi-directional earthquake excitations with increasing intensity. The acceleration response, roof displacement, inter-story drifts, residual drifts, shear force ratios, hysteresis curves, and local behaviour of the test specimen were analysed and evaluated. The results demonstrated that seismic performance of the test specimen was satisfactory in the plane of the shear wall; however, the structure sustained inter-story drift levels up to 2.45%. Negligible residual drifts were recorded after all applied earthquake excitations. Based on the shake-table test results, it is feasible to apply and popularize a self-centering precast RC frame with shear walls as a structural system in seismic regions.